pH-Specific Hydrothermal Assembly of Binary and Ternary Pb(II)-(O,N-Carboxylic Acid) Metal Organic Framework Compounds: Correlation of Aqueous Solution Speciation with Variable Dimensionality Solid-State Lattice Architecture and Spectroscopic Signatures

Hydrothermal pH-specific reactivity in the binary/ternary systems of Pb­(II) with the carboxylic acids N-hydroxyethyl-iminodiacetic acid (Heida), 1,3-diamino-2-hydroxypropane-N,N,N′,N′-tetraacetic acid (Dpot), and 1,10-phenanthroline (Phen) afforded the new well-defined crystalline compounds [Pb­(He...

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Veröffentlicht in:Inorganic chemistry 2012-09, Vol.51 (17), p.9282-9296
Hauptverfasser: Gabriel, C, Perikli, M, Raptopoulou, C. P, Terzis, A, Psycharis, V, Mateescu, C, Jakusch, T, Kiss, T, Bertmer, M, Salifoglou, A
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Sprache:eng
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Zusammenfassung:Hydrothermal pH-specific reactivity in the binary/ternary systems of Pb­(II) with the carboxylic acids N-hydroxyethyl-iminodiacetic acid (Heida), 1,3-diamino-2-hydroxypropane-N,N,N′,N′-tetraacetic acid (Dpot), and 1,10-phenanthroline (Phen) afforded the new well-defined crystalline compounds [Pb­(Heida)] n ·nH2O­(1), [Pb­(Phen)­(Heida)]·4H2O­(2), and [Pb3(NO3)­(Dpot)] n (3). All compounds were characterized by elemental analysis, FT-IR, solution or/and solid-state NMR, and single-crystal X-ray diffraction. The structures in 1–2 reveal the presence of a Pb­(II) center coordinated to one Heida ligand, with 1 exhibiting a two-dimensional (2D) lattice extending to a three-dimensional (3D) one through H-bonding interactions. The concurrent aqueous speciation study of the binary Pb­(II)–Heida system projects species complementing the synthetic efforts, thereby lending credence to a global structural speciation strategy in investigating binary/ternary Pb­(II)-Heida/Phen systems. The involvement of Phen in 2 projects the significance of nature and reactivity potential of N-aromatic chelators, disrupting the binary lattice in 1 and influencing the nature of the ultimately arising ternary 3D lattice. 3 is a ternary coordination polymer, where Pb­(II)-Dpot coordination leads to a 2D metal–organic-framework material with unique architecture. The collective physicochemical properties of 1–3 formulate the salient features of variable dimensionality metal–organic-framework lattices in binary/ternary Pb­(II)-(hydroxy-carboxylate) structures, based on which new Pb­(II) materials with distinct architecture and spectroscopic signature can be rationally designed and pursued synthetically.
ISSN:0020-1669
1520-510X
DOI:10.1021/ic300850g